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单斜相纳米氧化锆基低温SCR催化剂脱硝机制研究
摘要点击 2025  全文点击 1055  投稿时间:2014-09-15  修订日期:2014-10-21
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中文关键词  单斜相  纳米氧化锆  MnOx-CeO2/m-ZrO2催化剂  低温NH3-SCR  脱硝机制
英文关键词  monoclinic phase  nanocrystalline zirconium  MnOx-CeO2/m-ZrO2 catalysts  low-temperature NH3-SCR  denitration mechanism
作者单位E-mail
叶飞 南京师范大学地理科学学院, 江苏省物质循环与污染控制重点实验室, 南京 210023 15651909701@163.com 
刘荣 南京师范大学地理科学学院, 江苏省物质循环与污染控制重点实验室, 南京 210023 liurongle@163.com 
管昊 南京师范大学地理科学学院, 江苏省物质循环与污染控制重点实验室, 南京 210023  
贡湘君 南京师范大学地理科学学院, 江苏省物质循环与污染控制重点实验室, 南京 210023  
季凌晨 南京师范大学地理科学学院, 江苏省物质循环与污染控制重点实验室, 南京 210023  
中文摘要
      以纳米m-ZrO2为载体,用浸渍法制备出MnOx-CeO2/m-ZrO2催化剂,考察反应温度、活性组分负载量对催化剂NH3-SCR脱硝活性影响,探讨催化剂表面织构特征,分析催化剂脱硝活性机制. 结果表明,在低温脱硝温度范围,提高反应温度、增加活性组分负载量,有利于催化剂脱硝效率的增加. 110℃ 时,2.5%MnOx-CeO2/m-ZrO2脱硝效率为55.5%,15%MnOx-CeO2/m-ZrO2脱硝效率达93.5%. XRD、BET、XPS、H2-TPR表征结果表明,催化剂表面具有良好的氧化还原能力,表面织构对脱硝反应有利. NH3-TPD测试显示,MnOx-CeO2/m-ZrO2催化剂的脱硝反应机制为:NH3吸附在催化剂表面的Lewis酸性位和Brönsted酸性位上,通过反应生成相应中间产物NH2NO或NH4NO2,中间产物进一步分解最终转变为N2和H2O; 催化剂总脱硝反应效率中,在Lewis酸性位上的脱硝反应占比较大.
英文摘要
      The MnOx-CeO2/m-ZrO2 catalyst was prepared by impregnation with nano monoclinic-phase zirconium (m-ZrO2) as the supporter. The influence of active component and reaction temperature on the denitration performance of the catalyst was investigated, while the surface properties of the catalyst and the denitration mechanism were discussed. The denitration efficiency was improved as the active component increased and the reaction temperature rose. The denitration efficiency of 2.5% MnOx-CeO2/m-ZrO2 catalyst at 110℃ was 55.5% while that of 15% MnOx-CeO2/m-ZrO2 catalyst was 93.5%. The results of XRD, SEM, BET and H2-TPR showed that the surface structure of the loaded catalyst was beneficial for denitration and oxidation-reduction. NH3-TPD test demonstrated that NH3 was adsorbed at the Lewis acid sites and Brönsted acid sites on the surface of catalysts. Intermediate products NH2NO and NH4NO were generated from a series of reactions between NO and NH3 and finally transformed into N2 and H2O. Most of the denitration process happened at Lewis acid sites.

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